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Prevailing strategies typically rely on enhancing the \u03c0\u2010delocalization of molecular building blocks by cyclic polymerization. Here, we demonstrate a new approach\u2014simply connecting the \u03c0\u2010conjugated rings along a specific direction via linear polymerization. This concept is well exemplified by a novel hybrid crystal, BIQCdCl\n                    <jats:sub>4<\/jats:sub>\n                    (BIQ\u00a0=\u00a0C\n                    <jats:sub>18<\/jats:sub>\n                    H\n                    <jats:sub>14<\/jats:sub>\n                    N\n                    <jats:sub>2<\/jats:sub>\n                    , the protonated form of 2,2\u2032\u2010biquinoline). Although in accordance with H\u00fcckel's rule, the \u03c0\u2010electrons within two quinoline subunits are not fully delocalized over the entire BIQ molecule, this compound exhibits a record\u2010high birefringence value of \u0394\n                    <jats:italic>n<\/jats:italic>\n                    <jats:sub>exp<\/jats:sub>\n                    \u00a0=\u00a01.017@546 nm, surpassing all commercial birefringent crystals and many newly developed birefringent crystals, thereby setting a new benchmark for such materials. Detailed electronic structure investigation indicates that while the C\u2500C linkage limits \u03c0\u2010delocalization extension, linear polymerization enhances the disparity in the in\u2010plane (\n                    <jats:italic>X<\/jats:italic>\n                    ,\n                    <jats:italic>Y<\/jats:italic>\n                    ) \u03c0\u2010electron distribution, thereby maximizing the polarizability contrast between two specific polarization directions (i.e.,\n                    <jats:italic>Y<\/jats:italic>\n                    and\n                    <jats:italic>Z<\/jats:italic>\n                    ). This leads to exceptional polarizability anisotropy of the BIQ molecules, which, combined with their uniform alignment directed by [CdCl\n                    <jats:sub>4<\/jats:sub>\n                    ] tetrahedra and hydrogen bonding, ultimately results in the giant birefringence of BIQCdCl\n                    <jats:sub>4<\/jats:sub>\n                    .\n                  <\/jats:p>","DOI":"10.1002\/anie.202524729","type":"journal-article","created":{"date-parts":[[2026,1,27]],"date-time":"2026-01-27T13:59:56Z","timestamp":1769522396000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":13,"title":["Unveiling the Superior Birefringence Property of a Record\u2010Birefringent Crystal with Unique Building Block"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0009-0006-5393-9910","authenticated-orcid":false,"given":"Kaijie","family":"Xie","sequence":"first","affiliation":[{"name":"State Key Laboratory of Functional Crystal and Devices Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences  Fuzhou 350002 P.R. China"},{"name":"University of the Chinese Academy of Sciences  Beijing 100049 P.R. China"},{"name":"Fujian College University of Chinese Academy of Sciences  Fuzhou 35002 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0001-2776-9771","authenticated-orcid":false,"given":"Zhiyong","family":"Bai","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Functional Crystal and Devices Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences  Fuzhou 350002 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Weiqi","family":"Huang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Functional Crystal and Devices Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences  Fuzhou 350002 P.R. China"},{"name":"Fujian College University of Chinese Academy of Sciences  Fuzhou 35002 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ji","family":"Qi","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Functional Crystal and Devices Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences  Fuzhou 350002 P.R. China"},{"name":"Fujian College University of Chinese Academy of Sciences  Fuzhou 35002 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tingjuan","family":"Lin","sequence":"additional","affiliation":[{"name":"University of the Chinese Academy of Sciences  Beijing 100049 P.R. China"},{"name":"Fujian College University of Chinese Academy of Sciences  Fuzhou 35002 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Muhammad","family":"Zeeshan","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Functional Crystal and Devices Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences  Fuzhou 350002 P.R. China"},{"name":"University of the Chinese Academy of Sciences  Beijing 100049 P.R. China"},{"name":"Fujian College University of Chinese Academy of Sciences  Fuzhou 35002 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yanqiang","family":"Li","sequence":"additional","affiliation":[{"name":"Quantum Science Center of Guangdong\u2010Hong Kong\u2010Macao Greater Bay Area (Guangdong)  Shenzhen 518045 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yang","family":"Zhou","sequence":"additional","affiliation":[{"name":"Quantum Science Center of Guangdong\u2010Hong Kong\u2010Macao Greater Bay Area (Guangdong)  Shenzhen 518045 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Junhua","family":"Luo","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Functional Crystal and Devices Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences  Fuzhou 350002 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1190-684X","authenticated-orcid":false,"given":"Sangen","family":"Zhao","sequence":"additional","affiliation":[{"name":"Quantum Science Center of Guangdong\u2010Hong Kong\u2010Macao Greater Bay Area (Guangdong)  Shenzhen 518045 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,1,27]]},"reference":[{"key":"e_1_2_7_1_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41566\u2010021\u201000865\u20100"},{"key":"e_1_2_7_2_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41566\u2010022\u201000970\u20108"},{"key":"e_1_2_7_3_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41586\u2010018\u20100618\u20109"},{"key":"e_1_2_7_4_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.aax1839"},{"key":"e_1_2_7_5_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41566\u2010024\u201001501\u20103"},{"key":"e_1_2_7_6_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.aaw6747"},{"key":"e_1_2_7_7_1","doi-asserted-by":"publisher","DOI":"10.1016\/S0022-0248(98)00162-6"},{"key":"e_1_2_7_8_1","doi-asserted-by":"publisher","DOI":"10.1016\/S0030\u20104018(99)00091\u20107"},{"key":"e_1_2_7_9_1","doi-asserted-by":"publisher","DOI":"10.1364\/OL.31.000616"},{"key":"e_1_2_7_10_1","doi-asserted-by":"publisher","DOI":"10.1364\/JOSA.41.000416"},{"key":"e_1_2_7_11_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.ccr.2021.214380"},{"key":"e_1_2_7_12_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.inorgchem.4c05197"},{"key":"e_1_2_7_13_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.mtphys.2023.101197"},{"key":"e_1_2_7_14_1","doi-asserted-by":"publisher","DOI":"10.1039\/D3QM00225J"},{"key":"e_1_2_7_15_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.cjsc.2024.100304"},{"key":"e_1_2_7_16_1","doi-asserted-by":"publisher","DOI":"10.1002\/cjoc.70006"},{"key":"e_1_2_7_17_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202202746"},{"key":"e_1_2_7_18_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202403843"},{"key":"e_1_2_7_19_1","doi-asserted-by":"publisher","DOI":"10.1002\/cjoc.202401118"},{"key":"e_1_2_7_20_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202409336"},{"key":"e_1_2_7_21_1","doi-asserted-by":"publisher","DOI":"10.1002\/smll.202306158"},{"key":"e_1_2_7_22_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.newton.2025.100094"},{"key":"e_1_2_7_23_1","doi-asserted-by":"publisher","DOI":"10.1002\/smll.202304333"},{"key":"e_1_2_7_24_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.matt.2021.10.020"},{"key":"e_1_2_7_25_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201915094"},{"key":"e_1_2_7_26_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202424756"},{"key":"e_1_2_7_27_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.cjsc.2023.100044"},{"key":"e_1_2_7_28_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201407708"},{"key":"e_1_2_7_29_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.8b13280"},{"key":"e_1_2_7_30_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202211151"},{"key":"e_1_2_7_31_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.cgd.2c01050"},{"key":"e_1_2_7_32_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.inorgchem.3c00802"},{"key":"e_1_2_7_33_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202304498"},{"key":"e_1_2_7_34_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsami.2c15835"},{"key":"e_1_2_7_35_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202208811"},{"key":"e_1_2_7_36_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202504761"},{"key":"e_1_2_7_37_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.mattod.2025.04.008"},{"key":"e_1_2_7_38_1","doi-asserted-by":"publisher","DOI":"10.1039\/D4SC05756B"},{"key":"e_1_2_7_39_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.9b08851"},{"key":"e_1_2_7_40_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.8b10009"},{"key":"e_1_2_7_41_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41377-022-00941-2"},{"key":"e_1_2_7_42_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202506625"},{"key":"e_1_2_7_43_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.5c10200"},{"key":"e_1_2_7_44_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41566\u2010024\u201001461\u20108"},{"key":"e_1_2_7_45_1","unstructured":"The details of crystal structure data are listed in Tables S1\u2010S4. Deposition Numbers 2483340 contain the supplementary crystallographic data for this paper. These data are provided free of charge by the joint Cambridge Crystallographic Data Centre and Fachin\u2010formationszentrum Karlsruhe Access Structures service."},{"key":"e_1_2_7_46_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202303711"},{"key":"e_1_2_7_47_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202111604"},{"key":"e_1_2_7_48_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.4c01740"},{"key":"e_1_2_7_49_1","doi-asserted-by":"publisher","DOI":"10.1039\/D5SC01983D"},{"key":"e_1_2_7_50_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202509171"},{"key":"e_1_2_7_51_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja00179a045"},{"key":"e_1_2_7_52_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202011006"},{"key":"e_1_2_7_53_1","doi-asserted-by":"publisher","DOI":"10.1103\/PhysRevB.43.1993"},{"key":"e_1_2_7_54_1","doi-asserted-by":"publisher","DOI":"10.1063\/1.478401"}],"container-title":["Angewandte Chemie International Edition"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/pdf\/10.1002\/anie.202524729","content-type":"application\/pdf","content-version":"vor","intended-application":"text-mining"},{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/full-xml\/10.1002\/anie.202524729","content-type":"application\/xml","content-version":"vor","intended-application":"text-mining"},{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/pdf\/10.1002\/anie.202524729","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,9,23]],"date-time":"2026-09-23T16:57:40Z","timestamp":1790182660000},"score":1,"resource":{"primary":{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/10.1002\/anie.202524729"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2026,1,27]]},"references-count":54,"journal-issue":{"issue":"10","published-print":{"date-parts":[[2026,3,2]]}},"alternative-id":["10.1002\/anie.202524729"],"URL":"https:\/\/doi.org\/10.1002\/anie.202524729","archive":["Portico"],"relation":{},"ISSN":["1433-7851","1521-3773"],"issn-type":[{"value":"1433-7851","type":"print"},{"value":"1521-3773","type":"electronic"}],"subject":[],"published":{"date-parts":[[2026,1,27]]},"assertion":[{"value":"2025-11-09","order":0,"name":"received","label":"Received","group":{"name":"publication_history","label":"Publication History"}},{"value":"2026-01-16","order":2,"name":"accepted","label":"Accepted","group":{"name":"publication_history","label":"Publication History"}},{"value":"2026-01-27","order":3,"name":"published","label":"Published","group":{"name":"publication_history","label":"Publication History"}}],"article-number":"e24729"}}